Dataset Information

Templation and Concentration Drive Conversion Between a Fe^II₁₂L₁₂ Pseudoicosahedron, a Fe^II₄L₄ Tetrahedron, and a Fe^II₂L₃ Helicate.

ABSTRACT: We report the construction of three structurally distinct self-assembled architectures: Fe^II₁₂L₁₂ pseudoicosahedron 1, Fe^II₂L₃ helicate 2, and Fe^II₄L₄ tetrahedron 3, formed from a single triazatriangulenium subcomponent A under different reaction conditions. Pseudoicosahedral capsule 1 is the largest formed through subcomponent self-assembly to date, with an outer-sphere diameter of 5.4 nm and a cavity volume of 15 nm³. The outcome of self-assembly depended upon concentration, where the formation of pseudoicosahedron 1 was favored at higher concentrations, while helicate 2 exclusively formed at lower concentrations. The conversion of pseudoicosahedron 1 or helicate 2 into tetrahedron 3 occurred following the addition of a CB₁₁H₁₂^- or B₁₂F₁₂^2- template.

SUBMITTER: Zhang D

PROVIDER: S-EPMC9097479 | biostudies-literature | 2022 Jan

REPOSITORIES: biostudies-literature

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Publications

Templation and Concentration Drive Conversion Between a FeII12L12 Pseudoicosahedron, a FeII4L4 Tetrahedron, and a FeII2L3 Helicate.

Zhang Dawei D Gan Quan Q Plajer Alex J AJ Lavendomme Roy R Ronson Tanya K TK Lu Zifei Z Jensen Jesper D JD Laursen Bo W BW Nitschke Jonathan R JR

Journal of the American Chemical Society 20220111 3

We report the construction of three structurally distinct self-assembled architectures: FeII12L12 pseudoicosahedron 1, FeII2L3 helicate 2, and FeII4L4 tetrahedron 3, formed from a single triazatriangulenium subcomponent A under different reaction conditions. Pseudoicosahedral capsule 1 is the largest formed through subcomponent self-assembly to date, with an outer ...[more]

PMID: 35014803

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Project description:Rationale: Chemodynamic therapy (CDT) based on the Fe(II)-mediated Fenton reaction is an emerging tumor treatment strategy. However, the catalytic efficiency in tumors is crucially limited by Fe(II). Herein, an endogenous hydrogen sulfide (H2S) accelerated Fe(III)/Fe(II) transformation and photothermal synergistically enhanced CDT strategy based on ellagic acid-Fe-bovine serum albumin (EA-Fe@BSA) nanoparticles (NPs) was developed for colon tumor inhibition. On the one hand, the Fe(III) with low catalytic activity in the EA-Fe@BSA NPs could be rapidly reduced to the highly active Fe(II) by the abundant H2S in colon cancer tissues. Thus, a rapid Fe(III)/Fe(II) conversion system was established, wherein highly active Fe(II) ions were continuously regenerated to improve the CDT efficiency. On the other hand, the photothermal effect of EA-Fe@BSA NPs also accelerated the production of hydroxyl radicals (•OH), thereby synergistically enhancing the CDT performance and improving the therapeutic efficacy. Methods: The endogenous H2S accelerated Fe(III)/Fe(II) conversion and PTT enhanced CDT were investigated by characterization of the Fe valence state and detection of •OH. T 1-weighted magnetic resonance imaging (MRI) was tested both in vitro and in vivo. The biocompatibility of NPs were examined via MTT assay, hemolysis analysis and routine blood measurements. The enhanced CDT was investigated in HCT116 colon cancer cells by Calcein-AM/PI staining and MTT assay, and tumor inhibition was demonstrated in HCT116 tumor bearing mice. Results: In this work, EA-Fe@BSA NPs were constructed as a CDT theranostic reagent. The H2S accelerated Fe(III)/Fe(II) conversion was confirmed, more degradation of MB and generation of •OH demonstrated the enhanced CDT in vitro. EA-Fe@BSA NPs exhibited good T 1-weighted MRI performance. More importantly, it displayed strong near-infrared (NIR) absorption and excellent photothermal efficiency, further promotes the production of •OH. Hence, the efficacy of CDT was enhanced, and the tumor growth was inhibited efficiently. Conclusion: All results demonstrate that this strategy based on endogenous H2S promoted Fe(III)/Fe(II) transformation together with PTT acceleration permits efficient Fenton-reaction- mediated CDT both in vitro and in vivo, which holds great potential for effective colon cancer theranostics.

Dataset Information

Templation and Concentration Drive Conversion Between a Fe^II₁₂L₁₂ Pseudoicosahedron, a Fe^II₄L₄ Tetrahedron, and a Fe^II₂L₃ Helicate.

Publications

Templation and Concentration Drive Conversion Between a Fe<sup>II</sup><sub>12</sub>L<sub>12</sub> Pseudoicosahedron, a Fe<sup>II</sup><sub>4</sub>L<sub>4</sub> Tetrahedron, and a Fe<sup>II</sup><sub>2</sub>L<sub>3</sub> Helicate.

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